ABSTRACT
Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90[Formula: see text] ferroelectric) domain walls in the hybrid improper ferroelectric Ca[Formula: see text]Ti[Formula: see text]O[Formula: see text]. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.
ABSTRACT
Systems that exhibit phase competition, order parameter coexistence, and emergent order parameter topologies constitute a major part of modern condensed-matter physics. Here, by applying a range of characterization techniques, and simulations, we observe that in PbTiO3/SrTiO3 superlattices all of these effects can be found. By exploring superlattice period-, temperature- and field-dependent evolution of these structures, we observe several new features. First, it is possible to engineer phase coexistence mediated by a first-order phase transition between an emergent, low-temperature vortex phase with electric toroidal order and a high-temperature ferroelectric a1/a2 phase. At room temperature, the coexisting vortex and ferroelectric phases form a mesoscale, fibre-textured hierarchical superstructure. The vortex phase possesses an axial polarization, set by the net polarization of the surrounding ferroelectric domains, such that it possesses a multi-order-parameter state and belongs to a class of gyrotropic electrotoroidal compounds. Finally, application of electric fields to this mixed-phase system permits interconversion between the vortex and the ferroelectric phases concomitant with order-of-magnitude changes in piezoelectric and nonlinear optical responses. Our findings suggest new cross-coupled functionalities.
ABSTRACT
The goal of antenna design at optical frequencies is to deliver optical electromagnetic energy to loads in the form of, e.g., atoms, molecules or nanostructures, or to enhance the radiative emission from such structures, or both. A true optical antenna would, on a qualitatively new level, control the light-matter interaction on the nanoscale for controlled optical signal transduction, radiative decay engineering, quantum coherent control, and super-resolution microscopy, and provide unprecedented sensitivity in spectroscopy. Resonant metallic structures have successfully been designed to approach these goals. They are called optical antennas in analogy to radiofrequency (RF) antennas due to their capability to collect and control electromagnetic fields at optical frequencies. However, in contrast to the RF, where exact design rules for antennas, waveguides, and antenna-load matching in terms of their impedances are well established, substantial physical differences limit the simple extension of the RF concepts into the optical regime. Key distinctions include, for one, intrinsic material resonances including quantum state excitations (metals, metal oxides, semiconductor homo- and heterostructures) and extrinsic resonances (surface plasmon/phonon polaritons) at optical frequencies. Second, in the absence of discrete inductors, capacitors, and resistors, new design strategies must be developed to impedance match the antenna to the load, ultimately in the form of a vibrational, electronic, or spin excitation on the quantum level. Third, there is as yet a lack of standard performance metrics for characterizing, comparing and quantifying optical antenna performance. Therefore, optical antenna development is currently challenged at all the levels of design, fabrication, and characterization. Here we generalize the ideal antenna-load interaction at optical frequencies, characterized by three main steps: (i) far-field reception of a propagating mode exciting an antenna resonance, (ii) subsequent transformation of that mode into a nanoscale spatial localization, and (iii) near-field coupling via an enhanced local density of states to a quantum load. These three steps define the goal of efficient transformation of incident radiation into a quantum excitation in an impedance-matched fashion. We review the physical basis of the light-matter interaction at the transition from the RF to optical regime, discuss the extension of antenna theory as needed for the design of impedance-matched optical antenna-load coupled systems, and provide several examples of the state of the art in design strategies and suggest future extensions. We furthermore suggest new performance metrics based on the combination of electric vector field, field enhancement and capture cross section measurement to aid in comparison between different antenna designs and optimization of optical antenna performance within the physical parameter space.
ABSTRACT
We describe and demonstrate a new nanometer-scale broadband light source. It is based on the grating-coupled excitation of surface plasmon polaritons (SPPs) on the shaft of a sharp conical metal taper with a tip radius of few tens of nanometers. Far-field excitation of linear nanoslit gratings results in the resonant generation of SPPs traveling over more than 10 mum to the tip apex and converging to an intense radiative local light spot. Such nanofabricated tips are expected to find various applications in nanospectroscopy, overcoming problems with background illumination in apertureless microscopy.
